@article{62806, abstract = {{The electrical double‐layer plays a key role in important interfacial electrochemical processes from catalysis to energy storage and corrosion. Therefore, understanding its structure is crucial for the progress of sustainable technologies. We extract new physico‐chemical information on the capacitance and structure of the electrical double‐layer of platinum and gold nanoparticles at the molecular level, employing single nanoparticle electrochemistry. The charge storage ability of the solid/liquid interface is larger by one order‐of‐magnitude than predicted by the traditional mean‐field models of the double‐layer such as the Gouy–Chapman–Stern model. Performing molecular dynamics simulations, we investigate the possible relationship between the measured high capacitance and adsorption strength of the water adlayer formed at the metal surface. These insights may launch the active tuning of solid–solvent and solvent–solvent interactions as an innovative design strategy to transform energy technologies towards superior performance and sustainability.}}, author = {{Azimzadeh Sani, Mahnaz and Pavlopoulos, Nicholas G. and Pezzotti, Simone and Serva, Alessandra and Cignoni, Paolo and Linnemann, Julia and Salanne, Mathieu and Gaigeot, Marie‐Pierre and Tschulik, Kristina}}, issn = {{1433-7851}}, journal = {{Angewandte Chemie International Edition}}, keywords = {{single-entity electrochemistry, electrical double layer, supercapacitor, nanoparticles}}, number = {{5}}, publisher = {{Wiley}}, title = {{{Unexpectedly High Capacitance of the Metal Nanoparticle/Water Interface: Molecular‐Level Insights into the Electrical Double Layer}}}, doi = {{10.1002/anie.202112679}}, volume = {{61}}, year = {{2021}}, } @article{62805, abstract = {{Single-entity electrochemistry allows for assessing electrocatalytic activities of individual material entities such as nanoparticles (NPs). Thus, it becomes possible to consider intrinsic electrochemical properties of nanocatalysts when researching how activity relates to physical and structural material properties. Conversely, conventional electrochemical techniques provide a normalized sum current referring to a huge ensemble of NPs constituting, along with additives (e.g., binders), a complete catalyst-coated electrode. Accordingly, recording electrocatalytic responses of single NPs avoids interferences of ensemble effects and reduces the complexity of electrocatalytic processes, thus enabling detailed description and modelling. Herein, we present insights into the oxygen evolution catalysis at individual cubic Co3O4 NPs impacting microelectrodes of different support materials. Simulating diffusion at supported nanocubes, measured step current signals can be analyzed, providing edge lengths, corresponding size distributions, and interference-free turnover frequencies. The provided nano-impact investigation of (electro-)catalyst-support effects contradicts assumptions on a low number of highly active sites.}}, author = {{Liu, Zhibin and Corva, Manuel and Amin, Hatem M. A. and Blanc, Niclas and Linnemann, Julia and Tschulik, Kristina}}, issn = {{1422-0067}}, journal = {{International Journal of Molecular Sciences}}, keywords = {{electrocatalysis, oxygen evolution reaction, cobalt spinel, single-entity electrochemistry}}, number = {{23}}, publisher = {{MDPI AG}}, title = {{{Single Co3O4 Nanocubes Electrocatalyzing the Oxygen Evolution Reaction: Nano-Impact Insights into Intrinsic Activity and Support Effects}}}, doi = {{10.3390/ijms222313137}}, volume = {{22}}, year = {{2021}}, } @inbook{23733, author = {{Pollmeier, Pascal and Fechner, Sabine}}, booktitle = {{Lehrkräftebildung neu gedacht. Ein Praxishandbuch für die Lehre in den Naturwissenschaften und deren Didaktiken}}, editor = {{Kubsch, Marcus and Sorge, Stefan and Arnold, Julia and Graulich, Nicole}}, isbn = {{9783830943495}}, pages = {{150--154}}, publisher = {{Waxmann}}, title = {{{Förderung angehender Lehrkräfte im Umgang mit Evidenzen für den naturwissenschaftlichen Unterricht}}}, doi = {{10.31244/9783830993490}}, year = {{2021}}, } @inbook{27071, author = {{Pollmeier, Pascal and Fechner, Sabine}}, booktitle = {{Theorie und Praxis in der Lehrerbildung - Verhältnisbestimmungen aus der Perspektive von Fachdidaktiken}}, editor = {{Caruso, Carina and Harteis, Christian and Gröschner, Alexander}}, issn = {{2524-8677}}, publisher = {{Springer Fachmedien}}, title = {{{Zwischen den Stühlen? – Verknüpfung von Erfahrungen des Praxissemesters mit Theorien im Lehramtsstudium Chemie. Sukzessiven Kompetenzaufbau nach dem Praxissemester gestalten}}}, doi = {{10.1007/978-3-658-32568-8_16}}, year = {{2021}}, } @inbook{24935, author = {{Bauer, Anna and Sacher, Marc and Habig, Sebastian and Fechner, Sabine}}, booktitle = {{Hochschule auf Abstand. Ein multiperspektivischer Zugang zur digitalen Lehre}}, editor = {{Neiske, Iris and Osthushenrich, Judith and Schaper, Niclas and Trier, Ulrike and Vöing, Nerea}}, pages = {{155--168}}, publisher = {{ transcript Verlag}}, title = {{{Laborpraktika auf Distanz. Ansätze in den Naturwissenschaften}}}, doi = {{DOI: 10.14361/9783839456903-011}}, volume = {{3}}, year = {{2021}}, } @article{62851, abstract = {{To reduce high-level radiotoxic waste generated by nuclear power plants, highly selective separation agents for minor actinides are mandatory. The mixed N,O-donor ligand N,N,N′,N′-tetrakis[(6-carboxypyridin-2-yl)methyl]ethylenediamine (H4TPAEN; 1) has shown good performance as a masking agent in Am3+/Eu3+ separation studies. Adjustments on the pyridyl backbone to raise the hydrophilicity led to a decrease in selectivity and a decrease in M3+–Nam interactions. An enhanced basicity of the pyridyl N-donors was given as a cause. In this work, we examine whether a decrease in O-donor basicity can promote the M3+–Nam interactions. Therefore, we replace the deprotonated “charged” carboxylic acid groups of TPAEN4– by neutral amide groups and introduce N,N,N′,N’-tetrakis[(6-N″,N′′-diethylcarbamoylpyridin-2-yl)methyl]ethylenediamine (TPAMEN; 2) as a new ligand. TPAMEN was crystallized with Eu(OTf)3 and Eu(NO3)3·6H2O to form positively charged 1:1 [Eu(TPAMEN)]3+ complexes in the solid state. Alterations in the M–O/N bond distances are compared to [Eu(TPAEN)]− and investigated by DFT calculations to expose the differences in charge/energy density distributions at europium(III) and the donor functionalities of the TPAEN4– and TPAMEN. On the basis of estimations of the bond orders, atomic charges spin populations, and density of states in the Eu and potential Am and Cm complexes, the specific contributions of the donor–metal interaction are analyzed. The prediction of complex formation energy differences for the [M(TPAEN)]− and [M(TPAMEN)]3+ (M3+ = Eu3+, Am3+) complexes provide an outlook on the potential performance of TPAMEN in Am3+/Eu3+ separation.}}, author = {{Schnaars, Kathleen and Kaneko, Masashi and Fujisawa, Kiyoshi}}, issn = {{0020-1669}}, journal = {{Inorganic Chemistry}}, number = {{4}}, pages = {{2477--2491}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Effect of Oxygen-Donor Charge on Adjacent Nitrogen-Donor Interactions in Eu3+ Complexes of Mixed N,O-Donor Ligands Demonstrated on a 10-Fold [Eu(TPAMEN)]3+ Chelate Complex}}}, doi = {{10.1021/acs.inorgchem.0c03405}}, volume = {{60}}, year = {{2021}}, } @inproceedings{62965, author = {{Pollmeier, Pascal}}, keywords = {{Epistemologie, Mentale Modelle, Daten, Auswertung, Experiment}}, location = {{digital}}, title = {{{Epistemological enhancement through confrontation with anomalous data}}}, year = {{2021}}, } @inproceedings{62960, author = {{Pollmeier, Pascal}}, keywords = {{Epistemologie, Daten, anomale Daten}}, location = {{digital}}, title = {{{Epistemological enhancement t hrough confrontation with anomalous data}}}, year = {{2021}}, } @inproceedings{23758, author = {{Peeters, Hendrik and Habig, Sebastian and Fechner, Sabine}}, booktitle = {{Naturwissenschaftlicher Unterricht und Lehrerbildung im Umbruch?}}, editor = {{Habig, Sebastian}}, keywords = {{digitale Medien}}, pages = {{613--616}}, title = {{{Augmented Reality als Experimentierhilfe bei Beobachtung und Deutung}}}, volume = {{41}}, year = {{2021}}, } @article{64895, abstract = {{AbstractElektrochemische Synthese – Naturstoffe und deren Synthese – photokatalytische Redoxchemie – Farbstoffe – Nanostrukturen – Wirkstoffe – asymmetrische Katalyse und mehr.}}, author = {{Paradies, Jan and Andexer, Jennifer and Beifuss, Uwe and Beuerle, Florian and Brasholz, Malte and Breinbauer, Rolf and Ernst, Martin and Ganardi, Ruth and Gulder, Tobias A. M. and Hüttel, Wolfgang and Kath‐Schorr, Stephanie and Körber, Karsten and Kordes, Markus and Lehmann, Matthias and Lindel, Thomas and Luy, Burkhard and Mück‐Lichtenfeld, Christian and Muhle‐Goll, Claudia and Niemeyer, Jochen and Pfau, Roland and Pietruszka, Jörg and Röckl, Johannes L. and Schaschke, Norbert and Senge, Mathias O. and Straub, Bernd F. and Waldvogel, Siegfried R. and Werner, Thomas and Werz, Daniel B. and Winter, Christian}}, issn = {{1439-9598}}, journal = {{Nachrichten aus der Chemie}}, number = {{3}}, pages = {{38--68}}, publisher = {{Wiley}}, title = {{{Organische Chemie}}}, doi = {{10.1002/nadc.20214105947}}, volume = {{69}}, year = {{2021}}, } @article{65632, author = {{Zhuravlev, Evgeny and Milkereit, Benjamin and Yang, Bin and Heiland, Steffen and Vieth, Pascal and Voigt, Markus and Schaper, Mirko and Grundmeier, Guido and Schick, Christoph and Kessler, Olaf}}, issn = {{0264-1275}}, journal = {{Materials & Design}}, publisher = {{Elsevier BV}}, title = {{{Assessment of AlZnMgCu alloy powder modification for crack-free laser powder bed fusion by differential fast scanning calorimetry}}}, doi = {{10.1016/j.matdes.2021.109677}}, volume = {{204}}, year = {{2021}}, } @article{25301, author = {{Scherer, Beate and Kottenstedde, Ingo Leonard and Bremser, Wolfgang and Matysik, Frank-Michael}}, issn = {{0142-9418}}, journal = {{Polymer Testing}}, title = {{{Analytical characterization of polyamide 11 used in the context of selective laser sintering: Physico-chemical correlations}}}, doi = {{10.1016/j.polymertesting.2020.106786}}, year = {{2020}}, } @article{19679, abstract = {{In the present work, we provide an electronic structure based method for the “on-the-fly” determination of vibrational sum frequency generation (v-SFG) spectra. The predictive power of this scheme is demonstrated at the air-water interface. While the instantaneous fluctuations in dipole moment are obtained using the maximally localized Wannier functions, the fluctuations in polarizability are approximated to be proportional to the second moment of Wannier functions. The spectrum henceforth obtained captures the signatures of hydrogen bond stretching, bending, as well as low-frequency librational modes.}}, author = {{Ojha, Deepak and Kühne, Thomas D.}}, issn = {{1420-3049}}, journal = {{Molecules}}, title = {{{“On-The-Fly” Calculation of the Vibrational Sum-Frequency Generation Spectrum at the Air-Water Interface}}}, doi = {{10.3390/molecules25173939}}, volume = {{25}}, year = {{2020}}, } @article{19680, abstract = {{This is the second part of a project on the foundations of first-principle calculations of the electron transport in crystals at finite temperatures, aiming at a predictive first-principles platform that combines ab-initio molecular dynamics (AIMD) and a finite-temperature Kubo-formula with dissipation for thermally disordered crystalline phases. The latter are encoded in an ergodic dynamical system (Ω,G,dP), where Ω is the configuration space of the atomic degrees of freedom, G is the space group acting on Ω and dP is the ergodic Gibbs measure relative to the G-action. We first demonstrate how to pass from the continuum Kohn–Sham theory to a discrete atomic-orbitals based formalism without breaking the covariance of the physical observables w.r.t. (Ω,G,dP). Then we show how to implement the Kubo-formula, investigate its self-averaging property and derive an optimal finite-volume approximation for it. We also describe a numerical innovation that made possible AIMD simulations with longer orbits and elaborate on the details of our simulations. Lastly, we present numerical results on the transport coefficients of crystal silicon at different temperatures.}}, author = {{Kühne, Thomas and Heske, Julian Joachim and Prodan, Emil}}, issn = {{0003-4916}}, journal = {{Annals of Physics}}, pages = {{168290}}, title = {{{Disordered crystals from first principles II: Transport coefficients}}}, doi = {{https://doi.org/10.1016/j.aop.2020.168290}}, volume = {{421}}, year = {{2020}}, } @article{19681, author = {{Salem, M. Alaraby and Kühne, Thomas D.}}, issn = {{0026-8976}}, journal = {{Molecular Physics}}, pages = {{1--6}}, title = {{{Insight from energy decomposition analysis on a hydrogen-bond-mediated mechanism for on-water catalysis}}}, doi = {{10.1080/00268976.2020.1797920}}, year = {{2020}}, } @article{19823, abstract = {{Individual grains of chalcopyrite solar cell absorbers can facet in different crystallographic directions at their surfaces. To gain a deeper understanding of the junction formation in these devices, we correlate variations in the surface facet orientation with the defect electronic properties. We use a combined analytical approach based on scanning tunneling spectroscopy (STS), scanning electron microscopy, and electron back scatter diffraction (EBSD), where we perform these experiments on identical surface areas as small as 2 × 2 µm2 with a lateral resolution well below 50 nm. The topography of the absorber surfaces indicates two main morphological features: micro-faceted, long basalt-like columns and their short nano-faceted terminations. Our STS results reveal that the long columns exhibit spectral signatures typical for the presence of pronounced oxidation-induced surface dipoles in conjunction with an increased density of electronic defect levels. In contrast, the nano-faceted terminations of the basalt-like columns are largely passivated in terms of electronic defect levels within the band gap region. Corresponding crystallographic data based on EBSD experiments show that the surface of the basalt-like columns can be assigned to intrinsically polar facet orientations, while the passivated terminations are assigned to non-polar planes. Ab-initio calculations suggest that the polar surfaces are more prone to oxidation and resulting O-induced defects, in comparison to non-polar planes. Our results emphasize the correlation between morphology, surface facet orientations and surface electronic properties. Furthermore, this work aids in gaining a fundamental understanding of oxidation induced lateral inhomogeneities in view of the p-n junction formation in chalcopyrite thin-film solar cells.}}, author = {{Elizabeth, Amala and Conradi, Hauke and K. Sahoo, Sudhir and Kodalle, Tim and A. Kaufmann, Christian and Kühne, Thomas and Mirhosseini, Hossein and Abou-Ras, Daniel and Mönig, Harry}}, issn = {{1359-6454}}, journal = {{Acta Materialia}}, keywords = {{Chalcopyrite absorber, Scanning tunneling spectroscopy, Electron backscatter diffraction, Density functional theory, Surface dipole}}, title = {{{Correlating facet orientation, defect-level density and dipole layer formation at the surface of polycrystalline CuInSe2 thin films}}}, doi = {{https://doi.org/10.1016/j.actamat.2020.09.028}}, volume = {{200}}, year = {{2020}}, } @article{21239, abstract = {{The electrochemical nitrogen reduction reaction (NRR) to ammonia (NH3) is a promising alternative route for an NH3 synthesis at ambient conditions to the conventional high temperature and pressure Haber--Bosch process without the need for hydrogen gas. Single metal ions or atoms are attractive candidates for the catalytic activation of non-reactive nitrogen (N2), and for future targeted improvement of NRR catalysts, it is of utmost importance to get detailed insights into structure-performance relationships and mechanisms of N2 activation in such structures. Here, we report density functional theory studies on the NRR catalyzed by single Au and Fe atoms supported in graphitic C2N materials. Our results show that the metal atoms present in the structure of C2N are the reactive sites, which catalyze the aforesaid reaction by strong adsorption and activation of N2. We further demonstrate that a lower onset electrode potential is required for Fe--C2N than for Au--C2N. Thus, Fe--C2N is theoretically predicted to be a potentially better NRR catalyst at ambient conditions than Au--C2N owing to the larger adsorption energy of N2 molecules. Furthermore, we have experimentally shown that single sites of Au and Fe supported on nitrogen-doped porous carbon are indeed active NRR catalysts. However, in contrast to our theoretical results, the Au-based catalyst performed slightly better with a Faradaic efficiency (FE) of 10.1{\%} than the Fe-based catalyst with an FE of 8.4{\%} at −0.2 V vs. RHE. The DFT calculations suggest that this difference is due to the competitive hydrogen evolution reaction and higher desorption energy of ammonia.}}, author = {{Sahoo, Sudhir K. and Heske, Julian Joachim and Antonietti, Markus and Qin, Qing and Oschatz, Martin and Kühne, Thomas}}, journal = {{ACS Applied Energy Materials}}, number = {{10}}, pages = {{10061--10069}}, publisher = {{American Chemical Society}}, title = {{{Electrochemical N2 Reduction to Ammonia Using Single Au/Fe Atoms Supported on Nitrogen-Doped Porous Carbon}}}, doi = {{10.1021/acsaem.0c01740}}, volume = {{3}}, year = {{2020}}, } @article{17375, author = {{Zhou, Jiaqi and Khazaei, Mohammad and Ranjbar, Ahmad and Wang, Vei and Kühne, Thomas D. and Ohno, Kaoru and Kawazoe, Yoshiyuki and Liang, Yunye}}, journal = {{J. Mater. Chem. C}}, pages = {{5211--5221}}, publisher = {{The Royal Society of Chemistry}}, title = {{{Modulation of nearly free electron states in hydroxyl-functionalized MXenes: a first-principles study}}}, doi = {{10.1039/C9TC06837F}}, volume = {{8}}, year = {{2020}}, } @article{17379, author = {{Kumar Sahoo, Sudhir and Heske, Julian Joachim and Azadi, Sam and Zhang, Zhenzhe and V Tarakina, Nadezda and Oschatz, Martin and Z. Khaliullin, Rustam and Antonietti, Markus and Kühne, Thomas}}, journal = {{Scientific Reports}}, number = {{1}}, title = {{{On the Possibility of Helium Adsorption in Nitrogen Doped Graphitic Materials}}}, doi = {{10.1038/s41598-020-62638-z}}, volume = {{10}}, year = {{2020}}, } @article{17381, author = {{Elgabarty, Hossam and Kampfrath, Tobias and Bonthuis, Douwe Jan and Balos, Vasileios and Kaliannan, Naveen Kumar and Loche, Philip and Netz, Roland R. and Wolf, Martin and K{\, Thomas D. and Sajadi, Mohsen}}, journal = {{Science Advances}}, number = {{17}}, publisher = {{American Association for the Advancement of Science}}, title = {{{Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation}}}, doi = {{10.1126/sciadv.aay7074}}, volume = {{6}}, year = {{2020}}, }